Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination

doi:10.1016/j.cjche.2017.07.002

Chin.J.Chem.Eng. ›› 2018, Vol. 26 ›› Issue (2): 364-372.DOI: 10.1016/j.cjche.2017.07.002

• Process Systems Engineering and Process Safety • Previous Articles Next Articles

Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination

Chao Liu^1,2,3, Chenhui Liu^1,2,4, Jinhui Peng^1,2,3, Libo Zhang^1,2,3, Shixing Wang^1,2,3, Aiyuan Ma^1,2,3

1 State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming, 650093, China;
2 National Local Joint Laboratory of Engineering Application of Microwave Energy and Equipment Technology, Kunming, 650093, China;
3 Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming, 650093, China;
4 Key Laboratory of Resource Clean Conversion in Ethnic Regions, Education Department of Yunnan Province, Yunnan Minzu University, Kunming 650500, China

Received:2017-03-23 Revised:2017-07-04 Online:2018-03-16 Published:2018-02-28
Contact: Libo Zhang
Supported by:
Supported by the National Science Fund for Excellent Young Scholars of China (No. 51522405).

Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination

Chao Liu^1,2,3, Chenhui Liu^1,2,4, Jinhui Peng^1,2,3, Libo Zhang^1,2,3, Shixing Wang^1,2,3, Aiyuan Ma^1,2,3

1 State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Kunming University of Science and Technology, Kunming, 650093, China;
2 National Local Joint Laboratory of Engineering Application of Microwave Energy and Equipment Technology, Kunming, 650093, China;
3 Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming, 650093, China;
4 Key Laboratory of Resource Clean Conversion in Ethnic Regions, Education Department of Yunnan Province, Yunnan Minzu University, Kunming 650500, China

通讯作者: Libo Zhang
基金资助:
Supported by the National Science Fund for Excellent Young Scholars of China (No. 51522405).

Abstract

Abstract: Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO₂ and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl₂ caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.

Key words: Catalyst, Activated carbon, Deactivation, Mercuric chloride, Acetylene hydrochlorination, Carbon deposition

摘要： Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO₂ and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl₂ caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.

关键词: Catalyst, Activated carbon, Deactivation, Mercuric chloride, Acetylene hydrochlorination, Carbon deposition

Chao Liu, Chenhui Liu, Jinhui Peng, Libo Zhang, Shixing Wang, Aiyuan Ma. Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination[J]. Chin.J.Chem.Eng., 2018, 26(2): 364-372.

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Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination

Surface chemical characterization of deactivated low-level mercury catalysts for acetylene hydrochlorination

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